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For a small fraction of hot CO2 molecules immersed in a liquid-phase CO2 thermal bath, classical cavity molecular dynamics simulations show that forming collective vibrational strong coupling (VSC) between the C=O asymmetric stretch of CO2…

Chemical Physics · Physics 2021-05-11 Tao E. Li , Abraham Nitzan , Joseph E. Subotnik

Recent experiments have observed that the chemical and photophysical properties of molecules can be modified inside an optical Fabry-Perot microcavity under collective vibrational strong coupling (VSC) conditions, and such modification is…

Mesoscale and Nanoscale Physics · Physics 2021-03-09 Tao E. Li , Abraham Nitzan , Joseph E. Subotnik

Vibrational strong coupling (VSC) provides a novel means to modify chemical reactions and energy transfer pathways. To efficiently model chemical dynamics under VSC in the collective regime, herein a hybrid quantum mechanical/molecular…

Chemical Physics · Physics 2022-12-29 Tao E. Li , Sharon Hammes-Schiffer

Vibrational polaritons, hybrid light-matter states formed between molecular vibrations and infrared (IR) cavity modes, provide a novel approach for modifying chemical reaction pathways and energy transfer processes. For vibrational…

Chemical Physics · Physics 2025-05-16 Xinwei Ji , Tao E. Li

In vibrational strong coupling (VSC), molecular vibrations strongly interact with the modes of an optical cavity to form hybrid light-matter states known as vibrational polaritons. Experiments show that the kinetics of thermally activated…

Quantum Physics · Physics 2021-05-04 Matthew Du , Jorge A. Campos-Gonzalez-Angulo , Joel Yuen-Zhou

We assess the cavity molecular dynamics method for the calculation of vibrational polariton spectra, using liquid water as a specific example. We begin by disputing a recent suggestion that nuclear quantum effects may lead to a broadening…

Molecular polaritons, hybrid light-matter states resulting from strong cavity coupling of optical transitions, may provide a new route to guide chemical reactions. However, demonstrations of cavity-modified reactivity in clean benchmark…

Chemical Physics · Physics 2024-08-20 Liying Chen , Ashley P. Fidler , Alexander M. McKillop , Marissa L. Weichman

Recent experiments in polariton chemistry have demonstrated that reaction rates can be modified by vibrational strong coupling to an optical cavity mode. Importantly, this modification only occurs when the frequency of the cavity mode is…

Chemical Physics · Physics 2023-05-15 Marit R. Fiechter , Johan E. Runeson , Joseph E. Lawrence , Jeremy O. Richardson

Recent experiments have revealed the profound effect of strong light-matter interactions in optical cavities on the electronic ground state of molecular systems. This phenomenon, known as vibrational strong coupling (VSC), can modify…

Quantum Physics · Physics 2023-12-19 Thomas Schnappinger , Markus Kowalewski

Recent experiments and theory demonstrate that the the ground state properties and chemical reactivity of molecules can be modified inside an optical cavity. The vibrational strong or ultrastrong coupling results in the formation of…

Chemical Physics · Physics 2022-12-01 Qi Yu

We employ an exact quantum mechanical simulation technique to investigate a model of cavity-modified chemical reactions in the condensed phase. The model contains the coupling of the reaction coordinate to a generic solvent, cavity coupling…

Quantum Physics · Physics 2023-07-03 Lachlan P. Lindoy , Arkajit Mandal , David R. Reichman

Developing theoretical frameworks for vibrational strong coupling (VSC) beyond the single-mode approximation is crucial for a comprehensive understanding of experiments with planar Fabry-P\'erot cavities. Herein, a generalized cavity…

Chemical Physics · Physics 2024-06-18 Tao E. Li

Polariton chemistry may provide a new means to control molecular reactivity, permitting remote, reversible modification of reaction energetics, kinetics, and product yields. A considerable body of experimental and theoretical work has…

Chemical Physics · Physics 2023-10-26 Ashley P. Fidler , Liying Chen , Alexander M. McKillop , Marissa L. Weichman

We present a microscopic semi-analytical theory for the description of organic molecules interacting strongly with a cavity mode. Exciton-vibration coupling within the molecule and exciton-cavity interaction are treated on an equal footing…

Mesoscale and Nanoscale Physics · Physics 2016-11-15 Ning Wu , Johannes Feist , Francisco J. Garcia-Vidal

Polaritonic chemistry offers the possibility of modifying molecular properties and even influencing chemical reactivity through strong coupling between vibrational transitions and confined light modes in optical cavities. Despite…

Chemical Physics · Physics 2025-05-16 Thomas Schnappinger , Markus Kowalewski

Polaritons, mixed light-matter quasiparticles, undergo a transition to a condensed, macroscopically coherent state at low temperatures or high densities. Recent experiments show that coupling light to organic molecules inside a microcavity…

Quantum Gases · Physics 2014-03-06 Justyna A. Cwik , Sahinur Reja , Peter B. Littlewood , Jonathan Keeling

We simulate vibrational strong (VSC) and ultrastrong coupling (V-USC) for liquid water with classical molecular dynamics simulations. When the cavity modes are resonantly coupled to the O-H stretch mode of liquid water, the infrared…

Chemical Physics · Physics 2020-07-21 Tao E. Li , Joseph E. Subotnik , Abraham Nitzan

Polariton thermalization is a key process in achieving light-matter Bose--Einstein condensation, spanning from solid-state semiconductor microcavities at cryogenic temperatures to surface plasmon nanocavities with molecules at room…

We theoretically demonstrate that chemical reaction rate constant can be significantly suppressed by coupling molecular vibrations with an optical cavity, exhibiting both the collective coupling effect and the cavity-frequency modification…

Chemical Physics · Physics 2022-01-26 Arkajit Mandal , Xinyang Li , Pengfei Huo

A model designed to mimic the implications of the collective optical response of molecular ensembles in optical cavities on molecular vibronic dynamics is investigated. Strong molecule-radiation field coupling is often reached when a large…

Chemical Physics · Physics 2022-10-05 Bingyu Cui , Abraham Nitzan
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